CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jingyang Zhou,Ningning He,Pan He,Yang Li,Lijian Ma
The “two-in-one” strategy has been widely adopted for constructing diverse covalent organic frameworks (COFs) due to its excellent solvent adaptability. However, its reliance on simple single component reactions limits access to COFs with higher complexity and functionality. Herein, we integrated multicomponent reactions (MCRs) with the “two-in-one” strategy for the first time, fabricating three dual-linkage COFs (TAPQ-COF, 2,3-DHTAPQ-COF, and 2,5-DHTAPQ-COF) featuring compressed hexagonal pore structures. The concurrent presence of imine and imidazole linkages in the COF skeletons induced distinct crystallization pathways compared to counterparts with single linkage. Crucially, hydrogen bonding was found to modulate final crystallinity by influencing crystallization pathways. When applied to Ba 2+ /Pb 2+ separation—simulating the isolation of medical radionuclide 212 Pb from 224 Ra/ 212 Pb or 228 Ra/ 212 Pb generators—the isomeric 2,3-DHTAPQ-COF significantly outperformed 2,5-DHTAPQ-COF in adsorption performance. 2,3-DHTAPQ-COF exhibited exceptional selectivity for Pb 2+ (separation coefficient β Pb/Ba up to 54.2). Experimental and theoretical evidence revealed that the enhanced selectivity originates from the enhanced coordination ability of ortho-hydroxyl groups. This work ingeniously merges MCRs with the “two-in-one” strategy, expanding the structural diversity of COFs accessible through simplified synthesis and broadening the scope of MCR applications. The superior Ba 2+ /Pb 2+ separation capability of 2,3-DHTAPQ-COF provides new insights for designing COFs targeting medical radionuclide purification.
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高影响因子
COLLOID AND POLYMER SCIENCE
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2025
·
IF 2.3
Xiao Ting,Zou Wenjie,Tian Congzhong,Hu Wentao,He Jiancheng,Zhang Zhijun,Xu Chengyan,Zhou Fang
Flocculation technique is extensively adopted in the tackling of sulfide mineral processing wastewater, which contains abundant suspended solids and heavy metal ions. The functional groups of polymeric flocculants significantly influence the interactions between flocculants and pollutants. Herein, self-assembled monolayers (SAMs) terminated with − NH 2 , − OH, − COOH, and − CH 3 and in situ polymerization coating of acrylamide exclusively containing − CONH 2 were fabricated via the vapor-phase deposition, self-assembly molecular membrane, and atomic transfer radical polymerization methods. X-ray photoelectron spectroscopy, water contact angle measurements, and AFM imaging were utilized for the characterization of functionalized surfaces. The adsorption behavior of kaolin and Pb 2+ on these surfaces was explored using quartz crystal microbalance with dissipation (QCM-D). The amount of kaolin adsorbed on functionalized surfaces followed the sequence of − CONH 2 (∆ f of − 1360.55 Hz) > − NH 2 (∆ f of − 395.43 Hz) > − OH (∆ f of − 181.31 Hz) > − COOH (∆ f of − 1.75 Hz) > − CH 3 (∆ f of − 0.1 Hz). The polymer coating with acrylamide (CONH 2 -functionalized surface) with a specific molecular weight exhibited strong bridging effect, capturing quantities of kaolin. The amino group underwent protonation to form NH 3 + , combining with the negatively charged kaolin through electrostatic attraction. These indicated that both the bridging effect of flocculants and the electrical neutralization between flocculants and particles were critical factors influencing the settlement of kaolin. For Pb 2+ , its adsorption amount on functionalized surfaces followed the order of − COOH (∆ f of − 1.53 Hz) > − OH (∆ f of − 1.27 Hz) > − CH 3 (∆ f of − 0.34 Hz). The carboxyl group played a critical role in facilitating the adsorption of Pb 2+ through chelation and electrostatic interaction, confirming its function as an active site. Our findings provide profound insights into the structure–activity relationship of flocculants, underscoring the importance of designing efficient flocculants for wastewater treatment. Graphical
研究领域:
环境科学
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材料科学
·
化学工程
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Yuxin Xu,Yu Li,Guixin Wang,Meiling Zhang,Xiongxin Peng,Fan Yang,Kui Cheng
The effective mitigation of the environmental impact of heavy metal remains a significant scientific challenge. In this study, a novel and environmentally friendly approach has been proposed to fabricate three-dimensional (3D) functional composite materials for Pb(II) removal. The easy-to-recycle spherical adsorbent is prepared by the dual utilization of sodium alginate (SA) as a bio-source precursor for the synthesis of carbon dots (CDs) and as a natural framework for the formation of SA hydrogel. The abundant surface-active groups on the SA hydrogel not only provide additional adsorption sites for the aggregation of heavy metal ions but can also be readily cross-linked with CDs without chemical additives, and thereby offering a 3D porous structure for chelating metal ions. The resulting HL-5CDs adsorbent demonstrates an impressive adsorption capacity of 305.21 mg·g −1 for Pb(II). The adsorption mechanism involves both chemical reaction and diffusion, leveraging the porous structure and rich oxygen groups of the material. Notably, a pot experiment revealed that the as-prepared HL-5CDs could inhibit the bioavailability of Pb(II). This study introduces a green and straightforward method for creating high-performance adsorbents, showcasing potential applications in energy, cleaning, and the remediation of wastewater pollution.
研究领域:
环境科学
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材料科学
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SENSORS AND ACTUATORS B-CHEMICAL
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2017
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IF 5.401
Hongxu Guo,Zishan Zheng,Yanhui Zhang,Haibin Lin,Qingbo Xu
An amino-functionalized Ni(II)-based metal–organic framework (MOF), which employs 2-aminobenzenedicarboxylic acid as an organic linker, has been prepared by a simple one-pot hydrothermal reaction and characterized by Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). The prepared MOFs were found to be an effective material for the selective electrochemical detection of microgram levels of Pb 2+ in aqueous solution performed by square wave anodic stripping voltammetry. The electrochemical properties and applications of the modified electrode were also studied, in which operational parameters such as pH, deposition potential, and deposition time, were optimized to detect trace amounts of Pb 2+ ions. This method offers a new strategy for heavy metal detection using MOF materials.
研究领域:
材料科学
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分析化学
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高影响因子
BIORESOURCE TECHNOLOGY
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2020
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IF 7.539
Huabin Wang,Siqi Wang,Zhulei Chen,Xinquan Zhou,Jia Wang,Zhuqi Chen
Cationic and anionic heavy metal contaminants generally co-exist in practical industrial effluent, and simultaneously removal of these species is a bottleneck for most of the bio-adsorbents because of their contrary charge. In this work, pinewood sawdust derived engineered biochar (BC) was fabricated with MgAl layered double hydroxide (MgAl-LDH) nanosheets, which could efficiently and simultaneously capture heavy metal cations and oxyanions from wastewater. The synergetic effect between loaded MgAl-LDH and BC substantially improves its adsorption performance towards both cationic and anionic contaminants, i.e., Pb 2+ and CrO 4 2− . The adsorption capacity of MgAl-LDH/BC for Pb 2+ reached 591.2 mg/g, which is 263% higher than that of BC, and in the case of CrO 4 2− , the adsorption capacity is 330.8 mg/g, 416% higher than that of BC. The elimination of Pb 2+ was mainly attributed to forming complexations with surface functional groups. While for oxyanions removal, CrO 4 2− can be reduced to Cr 3+ by functional groups, and then generated Cr 3+ could replace Al 3+ via morphic substitution, consequently formed an MgCr-LDH structure. Further, in the continuous fixed-bed column study, 225 bed volume of simulating electroplating wastewater co-existed with Pb 2+ and CrO 4 2− can be efficiently treated. Hence, this study sheds light on the engineered biochar design to efficiently and simultaneously capture heavy metal cations and oxyanions and its feasibility on real wastewater purification.
研究领域:
环境科学
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材料科学
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Journal of Cleaner Production
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2023
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IF 11.1
Yuanjing Ding,Junkai Gao,Zhongzhi Chen,Qian He,Mengsheng Xia,Pengtao Xu,Yan Cao,Yan Chen
Based on the durability of fibroin and the biocompatibility of sericin, researchers are exploring ways to maximize their advantages by combining them in the biomedical field . Fortunately, silk cocoon shell (SC) offers a natural composite material of fibroin and sericin. However, the inherent hydrophobicity of SC, the random arrangement connection of fibers, and the protection provided by the outer sericin limit its application in purifying oil wastewater. In this work, a cost-effective method was developed to improve the hydrophilicity of SC and the mechanical properties of SC by utilizing obsoleted SC as a matrix as well as by dissolving portions of sericin proteins. The polydopamine particle (PDP) was utilized as the intermediate modification layer and a supramolecular gel (SMG) was introduced to the surface of SC, further improving the surface's hydrophilicity of SC. The study indicated that SC@P-SMG has excellent mechanical properties, favorable anti-fouling properties, and superior self-cleaning ability. Furthermore, when the SC@P-SMG was applied in water purification , it could achieve multifunctional applications such as purifying wastewater containing emulsified oil and Pb 2+ ions, methylene blue (MB), and oil-water mixture separation. This work provided innovative ideas to maximize the benefits of combining fibroin and sericin.
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Asia-Pacific Journal of Chemical Engineering
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2023
·Vol. 18
·期 5
·e2962
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IF 1.8
Tianming Yang,Xin Xin,Jin-Chi Jiang,Zhenhao Yin,Long-Yue Meng
The sensitive detection of heavy metal ions with high toxicity and mobility is extremely important for environmental monitoring. In this study, nitrogen-doped biochar (N-BC) was synthesized using waste mushroom bran as a raw material, and nitrogen atoms were successfully doped onto the surface of the biochar via a facile process using an activation-carbonation strategy. The functional groups on the surface of the biochar were enriched via doping, and the roughness of the biochar surface was significantly improved. Experimental results showed that N-BC was an efficient sensing material for electroanalysis; therefore, it was used to construct a novel electrochemical sensing platform. The electrochemical response of the biochar-modified working electrodes was effectively improved for the detection of heavy metals. Under optimized deposition potential, enrichment time, and pH, the N-BC-based sensing platform could detect Pb 2+ and Cd 2+ separately as well as simultaneously, indicating its significant potential for electrochemical sensing.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2023
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IF 4.4
Tai Ye,Haohao Chen,Long Bai,Min Yuan,Hui Cao,Liling Hao,Xiuxiu Wu,Fengqin Yin,Fei Xu
Due to the threat of lead pollution to health, environmental and food safety, developing simple and fast detection methods is highly required. Whereas, traditional single-mode probe suffers from limited application scenario. In this study, a colorimetric and fluorometric dual-mode probe for Pb 2+ determination was constructed by using bifunctional G-quadruplex-hemin complex. In this dual-mode probe, enzyme strand and substrate strand of 8–17 DNAzyme are labeled with G-quadruplex-hemin complex and fluorophore, respectively. In the absence of Pb 2+ , the self-assembly of enzyme strand and substrate strand inhibits intrinsic mimic peroxidase of G-quadruplex-hemin complex by base-pairing, which also quench the fluorescence via in proximity effect. When the DNAzyme is activated by Pb 2+ , the quenched fluorescence is restored as well as the inherent peroxidase mimetic activity, leading to dual signal output. Under optimal conditions, this dual-mode probe exhibit a good linear relationship between logarithm of Pb 2+ concentration and signal difference within the range from 1.5 nM to 20 nM and 0.5 nM to 10 nM for colorimetric and fluorescence mode, respectively. The detection limits for the corresponding mode were estimated to be 1.29 nM and 0.16 nM, respectively. This dual-mode probe also successfully applied for the spiked river water assay with satisfactory recovery in the range of 93.2 %–115.3 %. This work paves a new way for DNAzyme based dual-mode probe construction.
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PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Siyu Li,Weijun Shan,Ting Rao,Yanou Qi,Ying Xiong,Zhenning Lou,Haibiao Yu,Junshuo Cui,Xiaogeng Feng
Heavy metal ions (HMIs) are accumulative and toxic for the environment, causing one of the recognized social problems, while some metal ions have positive applications in the prognosis of diseases. Therefore, there is a necessity to achieve rapid, convenient, highly efficient determination of HMIs. In this work, a novel composite, CAU-17/CSG, consisting of CAU-17 and cellulose graphene (CSG) is synthesized via in situ growth method and serves as an effective electrochemical sensor. Taking advantages of the high catalytic activity of Bi in CAU-17 and the good synergy between CAU-17 and CSG , CAU-17/CSG exhibits excellent electrocatalytic activity to achieve individual and simultaneous detection of low concentrations of Zn 2+ , Cd 2+ and Pb 2+ in aqueous solutions. The limits of detection (LOD) for Zn 2+ , Cd 2+ and Pb 2+ are 0.029, 0.008 and 0.011 μM (S/N = 3), with linear ranges of 0.3–10, 0.01–2 and 0.03–2 μM, respectively. Meanwhile, the sensor exhibits good stability, reproducibility and anti-interference ability. As expected, CAU-17/CSG exhibits good accuracy in detecting metal ions in water and blood samples. Considering the simple preparation method, stable structure and excellent performance, the prepared composites will have great potential for environmental and biomedical applications.
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SENSORS AND ACTUATORS B-CHEMICAL
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2018
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IF 5.667
Jiao Wang,Ziying Zhang,Xia Gao,Xiaodong Lin,Yaqing Liu,Shuo Wang
Lead ion (Pb 2+ ) is known as a major non-degradable environmental pollutant and is quite harmful to human health. In our investigation, a novel ratiometric fluorescent nanosensor with DNA-AgNCs as single fluorophore has been successfully constructed for ultrasensitive and specific detection of Pb 2+ . The single-strand DNA templated silver nanoclusters present green emission, which can be converted into red emission after approaching a specific DNA segment by forming duplex with its complementary DNA strands (ds-DNA-AgNCs). The ds-DNA-AgNCs contains rA cleavage site of Pb 2+ -dependent DNAzyme configuration. In the presence of Pb 2+ , the specific DNA segment would be released from the ds-DNA-AgNCs, resulting in discoloration of DNA-AgNCs from red to green. Since Pb 2+ can successively cleave the rA site, the signal change from red to green emission is amplified. Thus, benefiting from the Pb 2+ -dependent DNAzyme and the charming properties of DNA-AgNCs, the proposed platform exhibits a good linear relationship from 0.001 nM to 10 nM with a detection limit of 1.0 pM for Pb 2+ determination, which is lower than most of the reported Pb 2+ biosensors. Moreover, this sensitive ratiometric fluorescent probe exhibits excellent selectivity toward Pb 2+ detection in real samples, such as lake water, tap water, and human serum samples, illustrating the huge potential applications for complicated samples in the future.
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JOURNAL OF MOLECULAR LIQUIDS
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2019
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IF 4.561
Qingmiao Wang,Lai Peng,Yuanyu Gong,Feifei Jia,Shaoxian Song,Yanmei Li
Because of the easy-separation, high specific surface areas and rich binding sites, magnetic MoS 2 with nanoscale architectures showed great potential in working as adsorbents for heavy metal ions . However, the general composites of nanoscale MoS 2 and Fe 3 O 4 suffered from the poor stability in acidic solution due to their entire exposures of Fe 3 O 4 to H + , which made it difficult to regenerate the used adsorbents by the general acid treatment. This work reported a facile approach to prepare Fe 3 O 4 @Polydopamine (PDA)-MoS 2 nanospheres via in-situ growth of MoS 2 on the PDA modified Fe 3 O 4 nanospheres. Fe 3 O 4 @PDA-MoS 2 nanospheres possessed a fast adsorption of 2.4076 g/mg·min (Initial concentration of Pb 2+ : 200 mg/L) and high adsorption capacity of 508.9 mg/g at 298 K to Pb 2+ . This was because the specific surface area of MoS 2 grown in-situ on Fe 3 O 4 @PDA was 7.6 times that of the pure MoS 2 , which significantly increased the binding sites of MoS 2 for heavy metal ions. In addition, the as-prepared nanocomposites exhibited not only easy-separation within 120 s by an external magnet, but also long-term stability in strong acid solutions as well as facile regeneration by general acid treatment. The tight PDA layers outside the Fe 3 O 4 nanospheres could work as not only a template for the formation of MoS 2 nanoflowers but also an efficient protective coating for the improvement of the stability of nanocomposites. The findings might open up the possibility of expanding the practical application of nanoadsorbent in environmental remediation.
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高影响因子
POWDER TECHNOLOGY
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2018
·
IF 3.23
Weiwei Chu,Zhenzhen Lu,Ruiqin Tan,Shihui Tang,Wei Xu,Weijie Song,Junhua Zhao
In this work, β-SrHPO 4 , Sr 3 (PO 4 ) 2 , and Sr 5 (PO 4 ) 3 (OH) (SrHAp) powders were successfully prepared by a controllable hydrothermal method and were utilized in removal of lead ion (Pb 2+ ). The effects of pH value, contact time and initial ion concentration on the immobilization of Pb 2+ were investigated systematically. Results showed that β-SrHPO 4 exhibited a capacity of 1438 ± 45 mg/g for Pb 2+ , while Sr 3 (PO 4 ) 2 and SrHAp showed values of 1223 ± 45 mg/g and 543 ± 45 mg/g respectively under the optimum conditions. The XRD , SEM and EDX results revealed that the mechanism of Pb 2+ immobilization by β-SrHPO 4 , Sr 3 (PO 4 ) 2 and SrHAp was mainly due to a process of dissolution and precipitation in the acidic solution. Comparing the immobilization behavior and capacities of β-SrHPO 4 , Sr 3 (PO 4 ) 2 and SrHAp for Pb 2+ removal, it is shown that β-SrHPO 4 is an effective and eco-friendly material for the removal of Pb 2+ from acidic aqueous solutions among strontium phosphates materials.
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